Exceptionally strong coupling of defect emission in hexagonal boron nitride to stacking sequences

Abstract Van der Waals structures present a unique opportunity for tailoring material interfaces and integrating photonic functionalities. By precisely manipulating the twist angle and stacking sequences, it is possible to elegantly tune and functionalize the electronic and optical properties of layered van der Waals structures. Among these materials, two-dimensional hexagonal boron nitride (hBN) stands out for its remarkable optical properties and wide band gap, making it a promising host for solid state single photon emitters at room temperature. Previous investigations have demonstrated the observation of bright single photon emission in hBN across a wide range of wavelengths. In this study, we unveil an application of van der Waals technology in modulating their spectral shapes and brightness by carefully controlling the stacking sequences and polytypes. Our theoretical analysis reveals remarkably large variations in the Huang-Rhys factors–an indicator of the interaction between a defect and its surrounding lattice–reaching up to a factor of 3.3 for the same defect in different stacking sequences. We provide insights into the underlying mechanism behind these variations, shedding light on the design principles necessary to achieve rational and precise control of defect emission. This work paves the way for enhancing defect identification and facilitating the engineering of highly efficient single photon sources and qubits using van der Waals materials.